Spin-Polarized Photocatalytic CO2Reduction of Mn-Doped Perovskite Nanoplates

Cheng Chieh Lin; Ting Ran Liu; Sin Rong Lin; Karunakara Moorthy Boopathi; Chun Hao Chiang; Wen Yen Tzeng; Wan Hsiu Chang Chien; Hua Shu Hsu; Chih Wei Luo; Hui Ying Tsai; Hsin An Chen; Pai Chia Kuo; Jessie Shiue; Jau Wern Chiou; Way Faung Pong; Chia Chun Chen; Chun Wei Chen

doi:10.1021/jacs.2c06060

Spin-Polarized Photocatalytic CO₂Reduction of Mn-Doped Perovskite Nanoplates

Cheng Chieh Lin, Ting Ran Liu, Sin Rong Lin, Karunakara Moorthy Boopathi, Chun Hao Chiang, Wen Yen Tzeng, Wan Hsiu Chang Chien, Hua Shu Hsu, Chih Wei Luo, Hui Ying Tsai, Hsin An Chen, Pai Chia Kuo, Jessie Shiue, Jau Wern Chiou, Way Faung Pong, Chia Chun Chen^*, Chun Wei Chen^*

^*Corresponding author for this work

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

170 Citations (Scopus)

Abstract

"Spin"has been recently reported as an important degree of electronic freedom to improve the performance of electrocatalysts and photocatalysts. This work demonstrates the manipulations of spin-polarized electrons in CsPbBr3 halide perovskite nanoplates (NPLs) to boost the photocatalytic CO2 reduction reaction (CO2RR) efficiencies by doping manganese cations (Mn2+) and applying an external magnetic field. Mn-doped CsPbBr3 (Mn-CsPbBr3) NPLs exhibit an outstanding photocatalytic CO2RR compared to pristine CsPbBr3 NPLs due to creating spin-polarized electrons after Mn doping. Notably, the photocatalytic CO2RR of Mn-CsPbBr3 NPLs is significantly enhanced by applying an external magnetic field. Mn-CsPbBr3 NPLs exhibit 5.7 times improved performance of photocatalytic CO2RR under a magnetic field of 300 mT with a permanent magnet compared to pristine CsPbBr3 NPLs. The corresponding mechanism is systematically investigated by magnetic circular dichroism spectroscopy, ultrafast transient absorption spectroscopy, and density functional theory simulation. The origin of enhanced photocatalytic CO2RR efficiencies of Mn-CsPbBr3 NPLs is due to the increased number of spin-polarized photoexcited carriers by synergistic doping of the magnetic elements and applying a magnetic field, resulting in prolonged carrier lifetime and suppressed charge recombination. Our result shows that manipulating spin-polarized electrons in photocatalytic semiconductors provides an effective strategy to boost photocatalytic CO2RR efficiencies.

Original language	English
Pages (from-to)	15718-15726
Number of pages	9
Journal	Journal of the American Chemical Society
Volume	144
Issue number	34
DOIs	https://doi.org/10.1021/jacs.2c06060
Publication status	Published - 2022 Aug 31

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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10.1021/jacs.2c06060

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Lin, C. C., Liu, T. R., Lin, S. R., Boopathi, K. M., Chiang, C. H., Tzeng, W. Y., Chien, W. H. C., Hsu, H. S., Luo, C. W., Tsai, H. Y., Chen, H. A., Kuo, P. C., Shiue, J., Chiou, J. W., Pong, W. F., Chen, C. C., & Chen, C. W. (2022). Spin-Polarized Photocatalytic CO₂Reduction of Mn-Doped Perovskite Nanoplates. Journal of the American Chemical Society, 144(34), 15718-15726. https://doi.org/10.1021/jacs.2c06060

Lin, CC, Liu, TR, Lin, SR, Boopathi, KM, Chiang, CH, Tzeng, WY, Chien, WHC, Hsu, HS, Luo, CW, Tsai, HY, Chen, HA, Kuo, PC, Shiue, J, Chiou, JW, Pong, WF, Chen, CC & Chen, CW 2022, 'Spin-Polarized Photocatalytic CO₂Reduction of Mn-Doped Perovskite Nanoplates', Journal of the American Chemical Society, vol. 144, no. 34, pp. 15718-15726. https://doi.org/10.1021/jacs.2c06060

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title = "Spin-Polarized Photocatalytic CO2Reduction of Mn-Doped Perovskite Nanoplates",

abstract = "{"}Spin{"}has been recently reported as an important degree of electronic freedom to improve the performance of electrocatalysts and photocatalysts. This work demonstrates the manipulations of spin-polarized electrons in CsPbBr3 halide perovskite nanoplates (NPLs) to boost the photocatalytic CO2 reduction reaction (CO2RR) efficiencies by doping manganese cations (Mn2+) and applying an external magnetic field. Mn-doped CsPbBr3 (Mn-CsPbBr3) NPLs exhibit an outstanding photocatalytic CO2RR compared to pristine CsPbBr3 NPLs due to creating spin-polarized electrons after Mn doping. Notably, the photocatalytic CO2RR of Mn-CsPbBr3 NPLs is significantly enhanced by applying an external magnetic field. Mn-CsPbBr3 NPLs exhibit 5.7 times improved performance of photocatalytic CO2RR under a magnetic field of 300 mT with a permanent magnet compared to pristine CsPbBr3 NPLs. The corresponding mechanism is systematically investigated by magnetic circular dichroism spectroscopy, ultrafast transient absorption spectroscopy, and density functional theory simulation. The origin of enhanced photocatalytic CO2RR efficiencies of Mn-CsPbBr3 NPLs is due to the increased number of spin-polarized photoexcited carriers by synergistic doping of the magnetic elements and applying a magnetic field, resulting in prolonged carrier lifetime and suppressed charge recombination. Our result shows that manipulating spin-polarized electrons in photocatalytic semiconductors provides an effective strategy to boost photocatalytic CO2RR efficiencies.",

author = "Lin, {Cheng Chieh} and Liu, {Ting Ran} and Lin, {Sin Rong} and Boopathi, {Karunakara Moorthy} and Chiang, {Chun Hao} and Tzeng, {Wen Yen} and Chien, {Wan Hsiu Chang} and Hsu, {Hua Shu} and Luo, {Chih Wei} and Tsai, {Hui Ying} and Chen, {Hsin An} and Kuo, {Pai Chia} and Jessie Shiue and Chiou, {Jau Wern} and Pong, {Way Faung} and Chen, {Chia Chun} and Chen, {Chun Wei}",

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year = "2022",

month = aug,

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doi = "10.1021/jacs.2c06060",

language = "English",

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T1 - Spin-Polarized Photocatalytic CO2Reduction of Mn-Doped Perovskite Nanoplates

AU - Lin, Cheng Chieh

AU - Liu, Ting Ran

AU - Lin, Sin Rong

AU - Boopathi, Karunakara Moorthy

AU - Chiang, Chun Hao

AU - Tzeng, Wen Yen

AU - Chien, Wan Hsiu Chang

AU - Hsu, Hua Shu

AU - Luo, Chih Wei

AU - Tsai, Hui Ying

AU - Chen, Hsin An

AU - Kuo, Pai Chia

AU - Shiue, Jessie

AU - Chiou, Jau Wern

AU - Pong, Way Faung

AU - Chen, Chia Chun

AU - Chen, Chun Wei

PY - 2022/8/31

Y1 - 2022/8/31

N2 - "Spin"has been recently reported as an important degree of electronic freedom to improve the performance of electrocatalysts and photocatalysts. This work demonstrates the manipulations of spin-polarized electrons in CsPbBr3 halide perovskite nanoplates (NPLs) to boost the photocatalytic CO2 reduction reaction (CO2RR) efficiencies by doping manganese cations (Mn2+) and applying an external magnetic field. Mn-doped CsPbBr3 (Mn-CsPbBr3) NPLs exhibit an outstanding photocatalytic CO2RR compared to pristine CsPbBr3 NPLs due to creating spin-polarized electrons after Mn doping. Notably, the photocatalytic CO2RR of Mn-CsPbBr3 NPLs is significantly enhanced by applying an external magnetic field. Mn-CsPbBr3 NPLs exhibit 5.7 times improved performance of photocatalytic CO2RR under a magnetic field of 300 mT with a permanent magnet compared to pristine CsPbBr3 NPLs. The corresponding mechanism is systematically investigated by magnetic circular dichroism spectroscopy, ultrafast transient absorption spectroscopy, and density functional theory simulation. The origin of enhanced photocatalytic CO2RR efficiencies of Mn-CsPbBr3 NPLs is due to the increased number of spin-polarized photoexcited carriers by synergistic doping of the magnetic elements and applying a magnetic field, resulting in prolonged carrier lifetime and suppressed charge recombination. Our result shows that manipulating spin-polarized electrons in photocatalytic semiconductors provides an effective strategy to boost photocatalytic CO2RR efficiencies.

AB - "Spin"has been recently reported as an important degree of electronic freedom to improve the performance of electrocatalysts and photocatalysts. This work demonstrates the manipulations of spin-polarized electrons in CsPbBr3 halide perovskite nanoplates (NPLs) to boost the photocatalytic CO2 reduction reaction (CO2RR) efficiencies by doping manganese cations (Mn2+) and applying an external magnetic field. Mn-doped CsPbBr3 (Mn-CsPbBr3) NPLs exhibit an outstanding photocatalytic CO2RR compared to pristine CsPbBr3 NPLs due to creating spin-polarized electrons after Mn doping. Notably, the photocatalytic CO2RR of Mn-CsPbBr3 NPLs is significantly enhanced by applying an external magnetic field. Mn-CsPbBr3 NPLs exhibit 5.7 times improved performance of photocatalytic CO2RR under a magnetic field of 300 mT with a permanent magnet compared to pristine CsPbBr3 NPLs. The corresponding mechanism is systematically investigated by magnetic circular dichroism spectroscopy, ultrafast transient absorption spectroscopy, and density functional theory simulation. The origin of enhanced photocatalytic CO2RR efficiencies of Mn-CsPbBr3 NPLs is due to the increased number of spin-polarized photoexcited carriers by synergistic doping of the magnetic elements and applying a magnetic field, resulting in prolonged carrier lifetime and suppressed charge recombination. Our result shows that manipulating spin-polarized electrons in photocatalytic semiconductors provides an effective strategy to boost photocatalytic CO2RR efficiencies.

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Spin-Polarized Photocatalytic CO₂Reduction of Mn-Doped Perovskite Nanoplates

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